The invention discloses a preparation method of a multilayer diamond-like film with high hardness, which comprises the following steps: a substrate is sputter cleaned, the diamond-like film is deposited by a depositing method with magnetic filtering and cathode vacuum arc, and the depositing method comprises steps of closing a vacuum chamber, vacuumizing the vacuum chamber to the pressure of 10<-3> Pa, turning on a pot lead cathode arc source, exerting negative bias voltage from minus 50 V to minus 200 V on the substrate and simultaneously and periodically letting in argon of 99.99 percent; furthermore, a control period lasts for 120 to 600 seconds, the time for letting in the argon is 10 to 50 percent of the control period, and the argon pressure in the vacuum chamber during argon inletting is 0.01 to 0.1 Pa; time for shutting off the argon is 90 to 50 percent of the control period, and the vacuum degree of the vacuum chamber at the time is 10<-4> to 10<-3> Pa; the number of the control periods is 3 to 50. The preparation method of the multilayer diamond-like film with high hardness has simple technique, low cost, produced films with strong bonding force, high hardness, large thickness, small stress and excellent mechanical and tribology performance; as well as wide application space in the industrial application field.